臺灣博碩士論文加值系統

過去公共衛生或健康風險評估對人體暴露於三鹵甲烷(trihalomethanes, THMs)的研究著重於飲用水的評估，相關的研究指出暴露於含三鹵甲烷的飲用水中三鹵甲烷的致癌風險為2.0×10-5 ~ 1.18×10-4，已超過美國環保署建議可接受的致癌風險(10-6)。游泳池的消毒方式與飲用水類似即加氯消毒，但游泳池的水是持續循環使用，使得加氯消毒所產生的消毒副產物容易累積在游泳池中。因此，相較於飲用水，游泳池水中三鹵甲烷的濃度可能較高，游泳者暴露於三鹵甲烷的風險亦可能較高。可惜針對游泳過程暴露三鹵甲烷的健康風險評估研究，目前仍相當有限，故需要針對游泳池環境中的三鹵甲烷進行檢測並進行健康風險評估。
目前已有許多游泳池環境監測的研究，但針對如何進行採樣包括三鹵甲烷在時間及空間上的差異進行探討，甚至有研究只取一個樣本即代表整個游泳池水中三鹵甲烷的濃度，此作法是否可合理的反應游泳池水中三鹵甲烷的實際狀況，有待更進一步的評估。所以需要了解游泳池水中三鹵甲烷的濃度在時間及空間上是否為均質，並探討影響三鹵甲烷濃度差異的素因。
本研究的研究目的：(1)分析國內游泳池環境中三鹵甲烷的濃度，以了解國人游泳過程中暴露的程度；(2)收集游泳池其他環境因子(餘氯量、總有機碳、游泳人數、溫度)，探討環境因子對水中三鹵甲烷的影響；(3)利用多暴露途徑(包括呼吸、皮膚接觸、攝食)的劑量模式，以蒙地卡羅模擬技術(Monte Carlo Simulation)，進行游泳者暴露三鹵甲烷的健康風險評估。
研究結果顯示：(1)本研究檢測五座室內游泳池，水中總三鹵甲烷濃度為6.39~22.15 μg/L，優勢物種為氯仿(占總三鹵甲烷55~95.2%)，若比照飲用水的污染物容許濃度標準(總三鹵甲烷: 100 μg/L)，並未超出管制標準；以模式推估空氣中總三鹵甲烷濃度為46.37~84.26 μg/m3。(2) 每座游泳池於3~4個不同的採樣點採集水樣，結果發現12次的採樣分析中，其中有9次採樣點之間水中三鹵甲烷的濃度並無顯著的差異。另外3次有差異的部份，發現與自由餘氯、總有機碳和單位時間游泳人次有關。自由餘氯量及總有機碳為形成三鹵甲烷前趨物質，故其濃度對水中三鹵甲烷濃度分佈，呈正向的影響；另外，單位時間游泳人次與三鹵甲烷濃度改變量呈正相關，發現游泳人次愈多時，水中三鹵甲烷濃度降低量亦愈多，推測可能是游泳活動造成的擾動及紊流，促使三鹵甲烷自水中揮發。故建議進行游泳池採樣的同時，應搭配採集水中自由餘氯及計算游泳人數。(3) 依據水中三鹵甲烷濃度及模式推估的空氣濃度，結合國人相關的暴露參數進行風險評估，結果顯示，游泳過程男性所承受的風險：2.09×10-6 ~1.95×10-4，女性：1.99×10-6 ~2.04×10-4，最主要的暴露途徑為呼吸(67.23-69.83%)，其次為皮膚接觸(30.07-32.68%)。游泳池為提供健身運動的場所，本研究的結果顯示游泳池環境暴露三鹵甲烷的風險超出可接受的範圍，故游泳池的管理建議選擇其他的消毒方式，如臭氧、紫外線，可達到消毒滅菌的效果，且不會產生致癌性的消毒副產物。增加換水的頻率或在循環系統中加入適當的過濾設備，皆能有效降低三鹵甲烷的生成。如此一來，便可提供民眾安全的運動場所，確實保護人體健康。

Several studies have assessed the potential cancer risk resulted from exposure to trihalomethanes (THMs) in drinking water. These studies show that the lifetime cancer risk range from 2.0×10-5 to 1.18×10-4. These values exceed the acceptable risk (10-6) set by USEPA. In general, swimming pool water is treated in a way similar to drinking water using chlorination to keep swimmers from infections caused by microbial pathogens. Usually, swimming pool water is almost entirely recirculated. It provides the opportunity for the disinfection by-product to accumulate in pool water. Accordingly, the THMs level in swimming pool maybe higher than that of drinking water. Hence, it is necessary to monitor the level of THMs in swimming pool water and assess the risk of swimmer expose to THMs.
Numerous studies have investigated the level of THMs in swimming pool water. However, most of them did not address the issue of variation of THMs level in the pool water due to spatial and temporal effect. Some of the studies even only took one sample to represent the THMs level in swimming pool. It might not reflect the actual level of THMs in the pool water. For this reason, further study is needed in order to understand the level of the variation.
The objectives of this study are: (1) to determine the level of THMs in the pool water so that the level of exposure can be estimated; (2) to collect data of other environmental factors in swimming pool (free available chlorine, total organ carbon, number of swimmers, and temperature of water), and to discuss the effect of environment factor associated with the THMs level in swimming pool water; (3) to develop a multi-pathway exposure model for the swimmers, and to study the cancer risk contribution from different exposure routes (oral ingestion, inhalation and dermal absorption).
The study results revealed that the THMs concentrations in five swimming pools ranged from 6.93 to 22.15 μg/L in water and from 46.37 to 84.26 μg/m3 in air. Chloroform was the dominate THMs species(55.0–95.2 %).
We have conducted 12 sets of sampling schsdules, three sets showed significantly difference for the levels of THMs taken at different sampling points. The difference was attributed to the level of free available chlorine, total organic carbon (TOC), and the number of swimmers per unit time. We found that free available chlorine and TOC were positively correlated to THMs levels in swimming pool water. In addition, number of swimmers per unit time had negative correlation with the level of THMs in water. This may be due to the fact that turbulence caused by swimmers might increase the rate of volatilization of THM from water to ambient air.
The lifetime cancer risk from exposure to THMs in swimming pool for males and females were in 2.09×10-6 –1.95×10-4 and 1.99×10-6 –2.04×10-4, respectively. The most important exposure pathway for swimmers was inhalation (67.23-69.83%), followed by dermal absorption (30.07-32.68%). Risk contribution from oral ingestion was insignificant in this study. In order to keep the risk of exposure to THMs at a minimum level, certain mitigation program, such as choose other disinfection agent (UV or ozone), frequent water change and circulation of pool water through an appropriate filtering system were strongly suggested.

誌謝.................................................. I
中文摘要.............................................III
Abstract..............................................VI
表目錄...............................................XII
圖目錄...............................................XIV
第一章 緒論
1-1 研究背景及研究動機.................................1
1-2 研究目的及重要性...................................5
第二章 文獻回顧
2-1 加氯消毒的原理與機制...............................8
2-2 消毒副產物的種類..................................10
2-3 游泳池中THMS生成的影響因子........................12
2-3-1 有機物質.......................................12
2-3-2 餘氯量.........................................12
2-3-3 溫度...........................................13
2-3-4 溴離子濃度.....................................13
2-3-5 反應時間.......................................13
2-3-6 游泳人數.......................................14
2-4 游泳池加氯消毒與三鹵甲烷的形成與濃度分布..........15
2-5 游泳者暴露三鹵甲烷的多重暴露途徑..................17
2-6 人體暴露於三鹵甲烷的健康風險評估..................20
2-6-1 毒理學資料及相關的流行病學調查.................20
2-6-2 可接受之風險...................................24
2-6-3 相關健康風險評估研究...........................25
2-7 游泳池相關研究的採樣方法..........................30
第三章 研究方法
3-1 研究問題..........................................32
3-2 研究內容及執行架構................................34
3-3 研究對象..........................................36
3-4 游泳池水中與空氣中三鹵甲烷採樣與實驗分析..........37
3-4-1 水樣採樣.......................................37
3-4-2 總有機碳.......................................42
3-4-3 相關參數的收集.................................43
3-5 研究假設及統計分析................................44
3-6 游泳池三鹵甲烷多暴露途徑之健康風險評估............45
3-6-1 暴露評估.......................................45
3-6-2 風險特性化.....................................53
3-6-3 蒙地卡羅不確定性分析...........................55
第四章 結果與討論
4-1 游泳池水中三鹵甲烷採樣結果分析....................57
4-1-1 採樣分析結果...................................57
4-1-2 模式推估之空氣中三鹵甲烷濃度...................60
4-1-3 游泳池水中三鹵甲烷物種組成.....................61
4-1-4 本研究三鹵甲烷濃度與其他相關研究比較...........63
4-2 環境因子對三鹵甲烷濃度的影響......................67
4-2-1 水中三鹵甲烷濃度時間上的變異及影響因素.........67
4-2-2 水中三鹵甲烷濃度空間上的變異及影響因素.........73
4-2-3 溫度對水中三鹵甲烷濃度的影響...................77
4-3 游泳池暴露三鹵甲烷之健康風險評估..................80
4-3-1 游泳暴露三鹵甲烷之終身致癌風險評估.............80
4-3-2 三鹵甲烷各物種對致癌風險之貢獻量...............81
4-3-3 各暴露途徑對致癌風險之貢獻量...................86
4-3-4 游泳暴露三鹵甲烷之非致癌風險評估...............90
4-3-5 游泳暴露三鹵甲烷之終身致癌風險之不確定性分析...91
4-3-6 游泳暴露三鹵甲烷終身致癌風險敏感度分析.........93
4-3-7 風險管理建議...................................96
第五章 結論與建議
5-1 結論.............................................100
5-2 研究限制.........................................104
5-3 建議 .............................................105
5-4 未來研究方向.....................................106
參考文獻..............................................107
附錄一 檢量線.........................................114
附錄二 水中三鹵甲烷分析之品質管制.....................117
附錄三 三鹵甲烷之液相傳輸係數(DL)、氣相傳輸係數(DG)及無因次之亨利常數(H).........................................118

Aggazzotti G, Fantuzzi G, Righi E, Predieri G. Blood and breath analyses as biological indicators of exposure to trihalomethanes in indoor swimming pools. The Science of Total Environmental 1998; 217: 155-163.
Aggazzotti G, Fantuzzi G, Righi E, Predieri G. Environmental and biological monitoring of chloroform in indoor swimming pools. Journal of Chromatography A 1995; 710: 181-190.
Aggazzotti G, Fantuzzi G, Righi E, Tartoni P, Cassindri T, Predieri G. Chloroform in alveolar air of individuals attending indoor swimming pools. Archives of Environmental Health 1993; 48: 250-254.
Aggazzotti G, Fantuzzi G, Tartoni PL, Predieri G. Plasma chloroform concentrations in swimmers using indoor swimming pools. Archives of Environmental Health 1990; 45: 175-179.
American Chemistry Council (ACC), An analysis of the training patterns and practices of competitive swimmers. Prepared by Richard Reiss, Sciences International Inc. 2002.
Batterman S, Huang A, Wang S, Zhang L. Reduction of ingestion exposure to trihalomethanes due to volatilization. Environmental Science and Technology 2000; 34: 4418-4424.
Blando JD, Cohn P. Exposure and health from swimming in outdoor pools contaminated by Trichloroethylene. Human and Ecological Risk Assessment 2004; 10: 717-731.
Bull RJ, Birnbaum LS, Cantor KP, Rose JB, Butterworth BE, Pegram R, Tuomisto J. Water chlorination: Essential process or cancer hazard. Fundamental and Applied Toxicology 1995; 28:155-166.
Cammann K, and H?佒ner K. Trihalomethane concentrations in swimmers’ and bath attendants’blood and urine after swimming or working in indoor swimming pools. Archives of Environmental Health 1995; 50: 61-65.
Cantor KP, Hoover R, Mason TJ, McCabe LJ. Associations of cancer mortality with halometnanes in drinking water. Journal of National Cancer Institute 1978; 61: 979-985.
Caro J, Gallego M. Assessment of exposure of workers and swimmers to trihalomethanes in an indoor swimming pool. Environmental Science and Technology 2007; 41: 4793-4798.
Corley RA, Gordon SM, Wallace LA. Physiologically Based Pharmacokinetic Modeling of the Temperature-Dependent Dermal Absorption of Chloroform by Humans following Bath Water Exposures. Toxicological Sciences 2000; 53: 13-23.
Corsi R, Howard CH. Volatilization rates from water to indoor air phase II. U.S.EPA Report. EPA 600/r-11/096, 2000.
Cotruvo JA. THMs in drinking water. Environmental Science and Technology 1981; 15: 268-274.
Erdinger L, K?伿n KP, Kirsch F, Feldhues R, Fr?爿el T, Noynek B, Gabrio T. Pathways of trihalomethane uptake in swimming pools. International Journal of Hygiene and Environmental Health 2004; 207: 571-575.
Fantuzzi G, Righi E, Predieri G, Ceppelli G, Gobba F, Aggazzotti G. Occupational exposure to trihalomethanes in indoor swimming pools. The Science of the Total Environment 2001; 264: 257-265.
Graham JD. Historical perspective of risk assessment in the federal government. Toxicology 1995; 102: 29-52.
Hsu CH, Jeng WL, Chang RM, Chien LC, Han BC. Estimation of potential lifetime cancer risks for trihalomethanes from consuming chlorinated drinking water in Taiwan. Environmental Research 2001; 85: 77-82.
Ichihashi K, Teranishi K, Ichimura A. Brominated trihalomethane formation in halogenation of humic acid in the coexistence of hypochlorite and hypobromite ions. Water Research 1999; 33: 477-483.
Jo WK, Weisel CP, Lioy PJ. Chloroform exposure and the health risk associated with multiple uses of chlorinated tap water. Risk analysis 1990; 10: 581-585.
Judd SJ, Black SH. Disinfection by-product formation in swimming pool waters: a simple mass balance. Water Research 2000; 34: 1611-1619.
Kavcar P, Odabasi M, Kitis M, Inal F, Sofuoglu SC. Occurrence, oral exposure and risk assessment of volatile organic compounds in drinking water for Izmir. Water Research 2006; 40: 3219-3230.
Kell KE, The Myth of 10-6 as a Definition of “Acceptable Risk”. Air and Waste Management Association, The 84th Annual Meeting and Exhibition; 1991.
Keskinen1 OP, Keskinen KL, Mero AA. Effect of Pool Length on Blood Lactate, Heart Rate, and Velocity in Swimming. International Journal of Sports Medicine 2007; 28: 407-413.
Kim H, Shim J, Lee S. Formation of disinfection by-products in chlorinated swimming pool water. Chemosphere 2002; 46: 123-130.
Knocke WR, West S, Hoehn RC. Effects of Low Temperature on the Removal of Trihalomethane Precursors by Coagulation. Journal of American Water Works Association 1986; 78: 189-196.
Kuo SW, Chiang TF, Lo II, Lai JS, Chan CC, Wang JD. Estimates of cancer risk from chloroform exposure during showering in Taiwan. The Science of the Total Environment. 1998; 218: 1-7.
Kuo SW, Chiang TF, Lo II, Lai JS, Chan CC, Wang JD. VOCs concentrations in Taiwan’s household drinking water. The Science of the Total Environment 1997; 208: 41-47.
Lee SC, Guo H, Lam SMJ, Lau SLA, Multipathway risk assessment on disinfection by-products of drinking water in Hong Kong. Environmental Research 2004; 94: 47-56.
Levesque B, Ayotte P, LeBlanc A, Dewailly E, PrudHomme D, Lavoie R, Allair S, Levallois P. Evaluation of dermal and respiratory chloroform exposures in humans. Environmental Health Perspectives 1993; 102: 1082-1087.
Lindstrom AB, Pleil JD, Berkoff DC. Alveolar breath sampling and analysis to assess trihalomethane exposures during competitive swimming training. Environmental Health Perspectives 1997; 105: 636-642.
Little JC. Applying the two-resistance theory to contaminant volatilization in showers. Environmental Science and Technology 1992; 26: 1341-1349.
Little JC, Chui N. Exposure to Contaminants in Drinking Water, CRC Press, Washington DC, 1998.
Mantel N, Bryan WR. Safety testing of carcinogens. Journal of the National Cancer Institute 1961; 27: 455-460.
Mazari-Hiriart M, Lopez-Vidal Y, Ponce-de-Leon S, Calva JJ, Rojo-Callejas F, Castillo-Rojas G. Longitudinal study of microbial diversity and seasonality in the Mexico city metropolitan area water supply system. Applied and Environmental Microbiology 2005; 71: 5129-5137.
McGeehin MA. Case-control study of bladder cancer and water disinfection methods in Colorado. American Journal of Epidemiology 1993; 138: 492-501.
Milot J, Rodriguez MJ, Serodes JB. Modeling the susceptibility of drinking water utilities to form high concentrations of trihalomethanes. Journal of Environmental Management 2000; 60: 155-171.
Morris RD, Audet AM. Chlorination, chlorination by-products and cancer: a meta-analysis. American Journal of Public Health 1992; 82: 955-963.
Moya J, Howard-Reed C, Corsi RL. Vlatilization of chemicals from tap water to indoor air from contaminated water used for showering. Environmental Science and Technology 1999; 33: 2321-2327.
Nazir M, Khan FI. Human health risk modeling for various exposure routes of trihalomethanes (THMs) in potable water supply. Environmental Modeling and Software 2006; 21: 1416-1429.
NTP (National Toxicology Program). NTP Technical Report on the Toxicology and Carcinogenesis Studies of Bromodichloromethane in F344/N Rats and B6C3F1 Mice (Gavage Studies). NTP Tech. Report Series No. 321. U.S. Dept. Health and Human Services, Public Health Service, National Institute of Health. 1987.
Percival RV, Miller AS, Schroeder CH, Leape JP. Environmental Regulation: Law, Science, and Policy; 2nd ed., Boston, Little, Brown, and Company, 1996.
Rodricks JV, and Taylor MR. Comparison of risk management in U.S. regulatory agencies. Journal of Hazardous Materials 1989; 21: 239-253.
Rodricks JV, Brett SM, Wrenn GC. Significant risk decisions in federal regulatory agencies. Regulatory Toxicology and Pharmacology 1987; 7: 307-320.
Shin D, Chung Y, Choi Y, Kim J, Park Y, Kum H. Assessment of disinfection by-products in drinking water in Korea. Journal of Exposure Analysis and Environmental Epidemiology 1999; 9: 192-199.
Singer PC. Humic substances as precursors for potentially harmful disinfection by-products. Water Science and Technology 1999; 40: 25-30.
Theiss JC, Stoner GD, Shimkin MB, Weisburger EK. Test for carcinogenicity of organic contaminants of United States drinking waters by pulmonary tumor response in strain a mice. Cancer Research 1977; 37: 2717-2720.
U.S. EPA. Final draft for the drinking water criteria document on trihalomethanes. Prepared for Health and Ecological Criteria Division, Office of Science and Technology, Washington, DC, 1994.
U.S. EPA, Developing Human Exposure Estimates for Individual DBPs, Draft Final Report. Washington, DC, 2003; 1-23.
U.S. EPA, Integrated Risk Information System, Available at: http://cfpub.epa.gov/ncea/iris/index.cfm. Accessed May 30, 2008.
U.S. EPA, National primary drinking water regulations: disinfectants and disinfection byproducts. Final Rule. Federal Register 1998. 63 :69406-69407.
U.S. EPA, The Risk Assessment Information System, Available at: http://rais.ornl.gov/. Accessed May 30, 2008.
U.S. EPA. (1998c) National primary drinking water regulations: disinfectants and disinfection byproducts. Final Rule. Federal Register 1998; 63: 69406-69407.
U.S. EPA., Exposure Factors Handbook, Volume III: Activity Factors. Office of Research and Development. Washington, DC, 1997; 15-16.
U.S. EPA., Swimmer exposure assessment model (SWIMODEL) Version 3.0, Washington, DC, 2003.
Uyak V. Multi-pathway risk assessment of trihalomethanes exposure in Istanbul drinking water supplies. Environment International 2006; 32: 12-21.
Uyak V, Toroz I, Meric S. Monitoring and modeling of trihalomethanes(THMs) for a water treatment plant in Istanbul. Desalination 2005; 176: 91-101.
Vahala R, Langvik VA, Laukkanen R. Controlling Adsorbable Organic Halogens (AOX) and Trihalomethanes (THM) Formation by Ozonation and Two-Step Granule. Water Science and Technology 1999; 40: 249-256.
Wang GS, Deng YC, Lin TF. Cancer risk assessment from trihalomethanes in drinking water. Science of the Total Environmental 2007; 387: 86-95.
Weisel CP, Shepard TA. Chloroform exposure and the body burden associated with swimming in chlorinated pools. In: Wang, RGM ed, Water Contamination and Health: Integration of Exposure Assessment Toxicology and Risk Assessment. Marcel Dekker, New York, 1994; 135-148.
White GG. Handbook of Chlorination and Alternative Disinfections, 3rd ed., Van Nostrand Reinhold, New York, 1992.
WHO. Guidelines for safe recreational water environments Vol 2: swimming pools and similar environments, Geneva, Switzerland. 2006.
內政部統計處。生命表, Available at: http://sowf.moi.gov.tw/stat/Life/List.html. 引用2008/5/30。
日本獨立法人化學物質風險管理研究中心. 日本暴露係數手冊, Available at: http://unit.aist.go.jp/crm/exposurefactors/index.htm. 引用2008/5/30。
余崇業，紫外光滅菌及加氯消毒處理對養豬廢水處理後放流水之再使用安全評估，碩士論文，台灣大學獸醫學研究所，台北市2000。
國民健康局。國民健康促進知識、態度與行為調查。2006年。
許惠悰：風險評估與風險管理。第二版。台北：新文京開發出版股份有限公司，2006；189-194。
勞工安全衛生研究所，物質安全資料表，Available at: http://www.iosh.gov.tw/msds.htm. 引用2008/5/30。
陳緯豪，游泳池水中含氯乙酸之生成及其液相光催化分解特性研究，碩士論文，高雄第一科技大學環境與安全衛生工程系，高雄市2006。
葉怡巖、陳偉銘、黃意潔、劉宇健、李漢鏗，自來水中三鹵甲烷風險評估程序之研究，中華民國環境工程學會第16屆年會，第29屆廢水處理技術研討會，國立成功大學，台南2004/11/26-2004/11/27。
鄧雅謓，飲用水中三鹵甲烷生成及其致癌風險評評估，碩士論文，台灣大學環境衛生研究所，台北市2003。
盧月詩，以氯及臭氧氧化模擬游泳池水質有機物之效能及消毒副產物之評估，碩士論文，逢甲大學環境工程與科學學系，台中市2005。
蕭美玲、林慶豐、陳惠芳、許明滿，「可接受風險」認知，藥物食品安全週報，行政院衛生署，2006/1/19。